2024 New's Items

A static quantum embedding scheme based on coupled cluster theory

Shee, A.
Faulstich, F. M.
Whaley, K. B.
Lin, L.
Head-Gordon, M.
2024

We develop a static quantum embedding scheme that utilizes different levels of approximations to coupled cluster (CC) theory for an active fragment region and its environment. To reduce the computational cost, we solve the local fragment problem using a high-level CC method and address the environment problem with a lower-level Møller–Plesset (MP) perturbative method. This embedding approach inherits many conceptual developments from the hybrid second-order Møller–Plesset (MP2) and CC works by Nooijen [J. Chem. Phys. 111, 10815 (1999)] and Bochevarov and Sherrill [J. Chem....

Evaluating Material Design Principles for Calcium-Ion Mobility in Intercalation Cathodes

Kim, J.
Sari, D.
Chen, Q.
Ceder, G.
Persson, K. A.
2024

Multivalent-ion batteries offer an alternative to Li-based technologies, with the potential for greater sustainability, improved safety, and higher energy density, primarily due to their rechargeable system featuring a passivating metal anode. Although a system based on the Ca2+/Ca couple is particularly attractive given the low electrochemical plating potential of Ca2+, the remaining challenge for a viable rechargeable Ca battery is to identify Ca cathodes with fast ion transport. In this work, a high-throughput computational pipeline is adapted to (1) discover...

The ab initio non-crystalline structure database: empowering machine learning to decode diffusivity

Zheng, H.
Sivonxay, E.
Christensen, R.
Gallant, M.
Luo, Z.
McDermott, M.
Huck, P.
Smedskjær, M. M.
Persson, K. A.
2024

Non-crystalline materials exhibit unique properties that make them suitable for various applications in science and technology, ranging from optical and electronic devices and solid-state batteries to protective coatings. However, data-driven exploration and design of non-crystalline materials is hampered by the absence of a comprehensive database covering a broad chemical space. In this work, we present the largest computed non-crystalline structure database to date, generated from systematic and accurate ab initio molecular dynamics (AIMD) calculations. We also show how the database can...

A Cellular Automaton Simulation for Predicting Phase Evolution in Solid-State Reactions

Gallant, M. C.
McDermott, M. J.
Li, B.
Persson, K. A.
2024

New computational tools for solid-state synthesis recipe design are needed in order to accelerate the experimental realization of novel functional materials proposed by high-throughput materials discovery workflows. This work contributes a cellular automaton simulation framework for predicting the time-dependent evolution of intermediate and product phases during solid-state reactions as a function of precursor choice and amount, reaction atmosphere, and heating profile. The simulation captures the effects of reactant particle spatial distribution, particle melting, and reaction atmosphere...

A dynamically bare metal interface enables reversible magnesium electrodeposition at 50 mAh cm2

Guha, R. D.
Vargas, S.
Spotte-Smith, E. W. C.
Epstein, A. R.
Venetos, M.
Kingsbury, R.
Wen, M.
Blau, S.
Persson, K. A.
2025

Understanding and facilitating pure magnesium nucleation/growth electrodeposition behavior with ultrahigh Coulombic efficiency is complicated by the phenomenon of solid electrolyte interphase (SEI) formation in state-of-the-art, halogen-free magnesium electrolytes. Defining the electrolyte properties necessary to achieve ideal electrodeposition/stripping (E/S) thus remains elusive. Here, we reveal for the first time, rapid magnesium electrodeposition behavior that forms densely aligned, micron-sized thin platelets by establishing a dynamic bare magnesium/electrolyte interface during high-...

Gold–Thiolate Nanocluster Dynamics and Intercluster Reactions Enabled by a Machine Learned Interatomic Potential

McCandler, C. A.
Pihlajamäki, A.
Malola, S.
Häkkinen, H.
Persson, K. A.
2024

Monolayer protected metal clusters comprise a rich class of molecular systems and are promising candidate materials for a variety of applications. While a growing number of protected nanoclusters have been synthesized and characterized in crystalline forms, their dynamical behavior in solution, including prenucleation cluster formation, is not well understood due to limitations both in characterization and first-principles modeling techniques. Recent advancements in machine-learned interatomic potentials are rapidly enabling the study of complex interactions such as dynamical behavior and...

Solubilities of Ethylene and Carbon Dioxide Gases in Lithium-Ion Battery Electrolyte

Soto, M.
Fink, K.
Zweifel, C.
Weddle, P. J.
Spotte-Smith, E. W. C.
Veith, G. M.
Persson, K. A.
Colclasure, A. M.
Tremolet de Villers, B. J.
2024

During Li-ion battery operation, (electro)chemical side reactions occur within the cell that can promote or degrade performance. These complex reactions produce byproducts in the solid, liquid, and gas phases. Studying byproducts in these three phases can help optimize battery lifetimes. To relate the measured gas-phase byproducts to species dissolved in the liquid-phase, equilibrium proprieties such as the Henry’s law constants are required. The present work implements a pressure decay experiment to determine the thermodynamic equilibrium concentrations between the gas and liquid phases...

The Role of Alkalis in Orchestrating Uranyl-Peroxide Reactivity Leading to Direct Air Capture of Carbon Dioxide

Arteaga, A.
Arino, T.
Moore, G. C.
Bustos, J. L.
Horton, M. K.
Persson, K. A.
Li, J.
Stickle, W. F.
Kohlgruber, T. A.
Surbella, R. G. III
Nyman, M.
2024

Spectator ions have known and emerging roles in aqueous metal-cation chemistry, respectively directing solubility, speciation, and reactivity. Here, we isolate and structurally characterize the last two metastable members of the alkali uranyl triperoxide series, the Rb+ and Cs+ salts (Cs-U1 and Rb-U1). We document their rapid solution polymerization via small-angle X-ray scattering, which is compared to the more stable Li+, Na+ and K+ analogues. To understand the role of the...

Overcoming systematic softening in universal machine learning interatomic potentials by fine-tuning

Deng, B.
Choi, Y.
Zhong, P.
Riebesell, J.
Anand, S.
Li, Z.
Jun, K.
Persson, K. A.
Ceder, G.
2024

Machine learning interatomic potentials (MLIPs) have introduced a new paradigm for atomic simulations. Recent advancements have seen the emergence of universal MLIPs (uMLIPs) that are pre-trained on diverse materials datasets, providing opportunities for both ready-to-use universal force fields and robust foundations for downstream machine learning refinements. However, their performance in extrapolating to out-of-distribution complex atomic environments remains unclear. In this study, we highlight a consistent potential energy surface (PES) softening effect in three uMLIPs: M3GNet, CHGNet...

Alkali-Ion-Assisted Activation of ε-VOPO4 as a Cathode Material for Mg-Ion Batteries

Sari, D.
Rutt, A.
Kim, J.
Chen, Q.
Hahn, N. T.
Kim, H.
Persson, K. A.
Ceder, G.
2025

Rechargeable multivalent-ion batteries are attractive alternatives to Li-ion batteries to mitigate their issues with metal resources and metal anodes. However, many challenges remain before they can be practically used due to the low solid-state mobility of multivalent ions. In this study, a promising material identified by high-throughput computational screening is investigated, ε-VOPO4, as a Mg cathode. The experimental and computational evaluation of ε-VOPO4 suggests that it may provide an energy density of >200 Wh kg−1 based on the average...